In 1956, the president of Tiffany & Co., Walter Hoving, asked Schlumberger to begin designing for the firm. He had his own workshop at the company until his retirement in the late 1970s and was eventually made a Vice-President.

Schlumberger's designs at Tiffany & Co. were remarkable for their whimsical interpretations of natural forms. He was especially inspired by sea creatures and other animals. Diana Vreeland wrote that Schlumberger "appreciates the miracle of jewels. For him, they are the ways and means to the realization of his dreams."