In a floor speech, Cruz accused his former Senate colleague of displaying a "shocking lack of sensitivity to the incendiary and damaging nature of his rhetoric."
"Mr. President, it is my belief that Secretary Kerry has thus proven himself unsuitable for his position and that before any further harm is done to our alliance with Israel, he should offer President Obama his resignation and the President should accept it," said Cruz, who was one of just 3 senators who voted against Kerry's confirmation to his post last year.
The conservative firebrand's remarks came on the same day that House Majority Leader Eric Cantor (R-VA), the only Jewish Republican in Congress, called on Kerry to apologize to Israelis and their government.
In a statement provided to TPM, State Department spokeswoman Jen Psaki explained his remarks about Israel and the Mid-East peace process, which is a high priority for Kerry.
"Secretary Kerry, like Justice Minister Livni, and previous Israeli Prime Ministers Olmert and Barak, was reiterating why there's no such thing as a one state solution if you believe, as he does, in the principle of a Jewish State," Psaki said. "He was talking about the kind of future Israel wants and the kind of future both Israelis and Palestinians would want to envision. The only way to have two nations and two peoples living side by side in peace and security is through a two state solution. And without a two state solution, the level of prosperity and security the Israeli and Palestinian people deserve isn't possible."