Zelensky, who is Jewish, made the appeal during an address to Israeli lawmakers, the latest in a series of speeches by videoconference to foreign legislatures.
In remarks that at several points compared Russian aggression to the Holocaust, Zelensky said that "Ukraine made the choice to save Jews 80 years ago."
"Now it's time for Israel to make its choice."
Israeli Prime Minister Naftali Bennett has walked a careful diplomatic line since Russia launched its invasion on February 24.
Stressing Israel's strong ties to Moscow and Kyiv, Bennett has sought to preserve delicate security cooperation with Russia, which has troops in Syria, across Israel's northern border.
Bennett has held regular phone calls with Zelensky and Russian President Vladimir Putin, including a three-hour meeting with Putin at the Kremlin on March 5.
While Ukrainian officials have voiced appreciation for Bennett's mediation efforts, Zelensky on Sunday implied that this too had proven to be a misstep.
"We can mediate between states but not between good and evil," the Ukrainian leader said.