The move comes 3½ months after The Wall Street Journal reported that many day-care centers listed on the site were unlicensed.
Michael Echenberg, executive vice president and finance chief at Care.com, resigned effective Aug. 30, the Waltham, Mass., company said in a Form 8-K filed with the Securities and Exchange Commission.
Michael Goss, vice president of finance, is expected to become acting chief financial officer, Care.com said in the filing.
Care.com shares closed 21% lower at $11.20.
The company, which started up in 2007, told the paper in a statement that Echenberg had taken a new opportunity. The Journal couldn't reach the executive for comment.
Care.com said last month it was implementing a number of enhanced safety measures on its consumer platform.
The steps included "in-depth background checks of caregivers and an identity verification pilot." It named Clark K. Ervin, former inspector general at both the Department of Homeland Security and the State Department, to the board.
That same day, Care.com reported a first-quarter loss of 5 cents a share against net income of 5 cents in the year-earlier period. Revenue rose 13% to $53.3 million.
Care.com's services include child care, senior care, pet care, housekeeping and others.