After splitting their time between London and the foothills of the Catskill Mountains for over 20 years, the celebrated British artists Gary Hume and Georgie Hopton are saying goodbye to their expansive estate in Accord, N.Y.

Ms. Hopton, 56, described the decades of having two lives — one fast-paced in a cosmopolitan city, another slow in a bucolic valley — as “truly magical.” Mr. Hume, 61, added, “It’s like cheating God.”

Mr. Hume and Ms. Hopton wouldn’t be selling, they said, if they were based in Manhattan. But traveling between London and Accord is a “palaver” they no longer want to deal with.

“It’s time for another dream,” Mr. Hume said.

The couple, who aren’t sure what that next dream will look like, are listing the 40-acre property for $4.25 million. They purchased the house and 30 acres for $453,500 in 2002, after becoming enamored with the area while visiting a friend in New Paltz. They bought an adjacent 10 acres in 2013 for $50,000. The listing agent is Megan Brenn-White of the Upstate Curious Team at Compass; annual taxes are $22,470.

Ms. Hopton and Mr. Hume could have chosen a second home in the English countryside years ago, but, as Ms. Hopton explained, they wanted to be “pioneers, not retirees.”

The dueling worlds they created have long been linked by their art. Mr. Hume, well known for his place in the Young British Artists movement of the late 1980s and ’90s, is acclaimed for his vibrant paintings on aluminum panels. Working in Accord has been a “great relief” for him. There, he said, “the culture — nature — doesn’t give a damn about your art.”

A similar dynamic has played out for Ms. Hopton. A Max Mara prize nominee in 2007, she has long been recognized for her engagement with diverse media, including sculpture, textiles, collage, printmaking and photography.

In London’s urban environment, Ms. Hopton mostly creates collages whose precision conveys the purpose that the city gives her. “There’s clarity in London,” she said.

“But in New York,” she added, “all the space makes everything questionable and possible.” Her art in Accord, more abstract and playful, involves painting with vegetables from her garden. A feeling of being “more connected to the universe” lends the art a transcendent quality.

The sprawling property, nestled in a little valley, includes structures dating to the mid-19th century, curated natural features, like ponds and meadows dotted with Mr. Hume’s sculptures (one a 15-foot white stainless-steel wheel, another a human-size limestone bud), a 2,300-square-foot home and Mr. Hume’s ultramodern studio, which the couple added in 2016.

Walking the paths that Mr. Hume cleared using the canopy as his guide, or sitting on the stone patio overlooking one of the ponds adorned with lily pads and listening to the splash of a small waterfall, there’s a feeling that you could be on either side of the Atlantic — in the Catskills or Giverny. There’s no sign of the road, and those extra 10 acres mean the undomesticated view is here to stay.

The house’s layout and windows capitalize on these views. The dining room and kitchen, equipped with Miele appliances, marble countertops and a copper island, look out at the peace of meadows and woods. Both the family room, off the dining room, and the screened-in porch adjacent to it have a wood-burning fireplace, as does the den on the other side of the first floor.

The home has three bedrooms upstairs, two smaller ones and a 550-square-foot primary suite with a large bathroom, a hallway lined with five closets and a view that Ms. Hopton described waking up to as “heaven.”

The house was built in 1860, and when the couple decided to expand it in 2012, they didn’t want to lose its rustic charm. Working with a local architect, Kurt Sutherland, they were able to keep the house’s cozy feeling even as they doubled its square footage, adding a primary bedroom, an open-plan living, dining, and kitchen area and windows overlooking a newly dug pond.

The house remains welcoming. As the clothesline strung with a pair of paint-splattered jeans attests, there’s little grandiosity there.

Beyond the home, there are many other impressive buildings, including a large barn still filled with hay from when the couple kept goats years ago, and still equipped with previous owners’ cow-milking instruments. The couple has often hosted dinner parties there, a cavernous space where light spills through a 15-by-20-foot entrance.

The property also has a chicken coop that is nearly 50 yards long and that Mr. Hume said was built in the early 1940s by Swiss Jews who had fled the Nazis. Another coop is now “the sugar shack,” where the couple makes maple syrup after tapping trees on the property. A garden, tiered with stones and full of butterflies and flowering rocket, is next to a cedar sauna. Jumping into the pond after a sauna session is a treasured ritual.

The most striking feature of the property is Mr. Hume’s 4,500-square-foot, two-story studio. With Corten steel siding, shuttered concrete inspired by the Hayward Gallery in London, a wall of windows on the lower level and towering ceilings and northern light upstairs, the space feels like a contemporary museum. It’s sparsely decorated because Mr. Hume is a messy worker. “To make an omelet, you’ve got to break some eggs,” he said.

Ms. Hopton’s studio is a short distance away, down a landscaped flight of steps. It’s bright and airy with a ceiling over 20 feet tall and pine shiplap walls. The studio where she used to work is a guesthouse.

With a rare combination of breathtaking scenery and antique charm juxtaposed with Mr. Hume’s studio, this will be “more like selling art than selling a home,” Ms. Brenn-White said. “There are a lot of intangible qualities that can’t be appraised.”