In 1948, he married Anne Beloff-Chain, sister of Renee Soskin, Max Beloff, John Beloff and Nora Beloff, and a biochemist of significant standing herself. In his later life, his Jewish identity became increasingly important to him. Chain was an ardent Zionist and he became a member of the board of governors of the Weizmann Institute of Science at Rehovot in 1954, and later a member of the executive council. He raised his children securely within the Jewish faith, arranging much extracurricular tuition for them. His views were expressed most clearly in his speech 'Why I am a Jew' given at the World Jewish Congress Conference of Intellectuals in 1965.