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|Mercedes unveiled its new Formula E car in Frankfurt. (AFP/Tobias SCHWARZ)|
The German manufacturer has dominated Formula One in recent years, winning five successive drivers' and constructors' world title doubles.
"We are embarking on a new mission, an electric mission," said Wolff at the presentation of the Mercedes-Benz EQ Silver Arrow 01.
Formula E will be entering its sixth season this year, with Frenchman Jean-Eric Vergne the defending drivers' champion.
Mercedes, who join Porsche as a new entry for the upcoming season, have named former McLaren F1 driver Vandoorne and current Formula Two championship leader De Vries as their two drivers.
"We are opening a new chapter," Wolff told AFP. "This is the first time we have an all-electric car, and it's a very special moment."
"Our goal is to reach a position that allows us to fight for race or championship wins, but the first season is about learning," he added at the presentation.
"We are newcomers, we must be modest."
Dutchman De Vries has claimed three wins in Formula Two this season for Red Bull Ring, and leads the drivers' standings by 59 points.
Belgium's Vandoorne collected 26 points from his three campaigns in F1 with McLaren from 2016-2018.
"I'm looking forward to driving for the same team as Stoffel," said the 24-year-old De Vries. "He has a lot of experience and is a great driver."
Vandoorne said: "The potential is huge and I simply can't wait to get started. It's going to be a big challenge, but I'm looking forward to it with confidence."
Wolff said that he believes the presence of historic constructors such as Mercedes, Porsche and BMW on the grid will help boost Formula E's profile.
"With the commitments of manufacturers comes great marketing force," he said. "The platform is already developing very well, but with the arrival of Porsche and Mercedes this year alongside Audi and BMW, the series will receive an extra boost."
Mercedes only returned to Formula One with a fully-fledged team after a 55-year absence in 2010.