David Eisner was a senior executive at the high-flying Internet company AOL in the late 1990s and early 2000s before he was tapped by then-President George W. Bush to run the $1-billion Corporation for National and Community Service.

He left that post in 2008 to make room for the next appointee and moved into the top spot at the National Constitution Center, a federally established museum in Philadelphia with a budget of less than $20-million.

Now, Mr. Eisner has taken the helm of a small religious nonprofit with just over $6-million to spend this year. He is the new chief executive of Repair the World, a New York organization aimed at mobilizing Jewish volunteers across the country.

His career path, he says, reflects a growing trend among people in their 50s and 60s.

“They are moving from success to significance,” says Mr. Eisner, 52, “shifting the size of their portfolio to focus on intensity and outcome.”

Often, he adds, their efforts, like his, are “framed around entrepreneurship and impact.”

Repair the World itself reframed in that mode in 2009, growing out of a mostly moribund one- or two-employee trade association of Jewish volunteer organizations.

The group changed its name from the Jewish Coalition for Services, broadened its mission and programs, and attracted new foundation support. It also introduced itself to Mr. Eisner, hoping to hire him as the first CEO of the repurposed group.

Mr. Eisner demurred, but he says that Repair the World “always stayed in the back of my mind” and that when he resigned from the National Constitution Center last year at the end of his three-year contract, he took notice of the Jewish group’s “strong brand and expertise in the field.”

“I wanted to jump back into the service world,” Mr. Eisner says.

Not only does working with the group allow him to connect more deeply than ever with his Jewish identity, he says, it also gives him a foothold in the broader world of faith-inspired nonprofits.

That might help him find solutions to one of the biggest challenges he says he faced at the Corporation for National and Community Service: Trying to more powerfully link religious organizations into the national service movement.

“If we could make stronger, better, and more sustainable connections on all sides, we’ll create an explosion of capacity in the volunteer field,” he says.

Geoff Lieberthal, chairman of Repair the World’s board, writes in an e-mail that trying to recruit Mr. Eisner again for the top job was “an easy choice.”

“David is a charismatic national leader in volunteering and service, with extensive experience in nonprofit, for-profit, government, and grant-making sectors,” writes Mr. Lieberthal, a principal at Lee Equity Partners, a private equity firm in New York.

“Repair the World has spent its first three years experimenting and growing,” he adds. “Now we are entering an exciting new phase to build a broad-based Jewish service movement and we think David has the track record, depth of knowledge, and experience to take Repair the World to a whole new level.”

In the next 100 days, Mr. Eisner says he is hoping to make two sets of announcements: one about a new strategic plan and another about the group’s plans to diversify sources of revenue.

The four grant makers that gave money to establish Repair the World—the Einhorn Family Charitable Trust, the Nathan Cummings Foundation, the Jim Joseph Foundation, and the Charles and Lynn Schusterman Family Foundation—still account for nearly all of its support (88 percent of last year’s budget).

Mr. Eisner sees a strong and passionate audience for Repair the World’s work, ready to be tapped. “We are moving beyond articulating our space and to getting things done,” he says.