Lawrence, 25, has never captained a team in a professional T20 fixture and his leadership experience extends to one Championship match for Essex and a warm-up match for England Lions in Abu Dhabi earlier this winter.
He was retained for the 2023 season on a £75,000 contract, and will receive a £10,000 bonus as captain.
"It's a real honour to be asked to captain this side," Lawrence said. "Following on from England's greatest white-ball captain is a huge challenge, but one I'm really excited to be taking on."
Spirit's men finished third in the Hundred last summer, losing the eliminator against Manchester Originals at the Ageas Bowl. They have retained most of their squad and will make three signings in Thursday evening's draft, including one overseas player.
"We've got a talented group of players coming back this season, and it's a great chance to build on last year's strong performance," Lawrence added. "I can't wait to lead the team out in front of a packed ground at Lord's."
Fraser Stewart, Spirit's general manager, said: "We are delighted that Dan has agreed to captain London Spirit's men's team this year. He is tactically astute and is a very popular and respected member of the dressing room.
"It's also pleasing that he's a local player from one of our partner counties, Essex, whose fans we hope will come to Lord's to support Dan and the London Spirit teams."
The Hundred runs from August 1-27 this summer, and has a standalone window which does not clash with any England international fixtures - men's or women's - for the first time.