The move comes amid ongoing structural changes at the London agency, with the integrating of its existing consumer and corporate teams under the plan announced by CEO Arlo Brady in October 2017, along with several new hires.
In a statement, Brady said: "After 14 years at Freuds – much of it at the top table – Caroline has decided she is ready for a change and will be leaving us at the end of June.
"During her time here Caroline has made a huge contribution, working with some of our biggest clients, driving new business and leading teams as the agency has changed and evolved. We wish her the very best."
She was previously associate director at Edelman before joining Freuds, where she has worked on major accounts including Unilever, AMEX, (RED), Pepsico, Evian, KFC and Sainsbury’s.
Grierson, meanwhile, is set to leave in July after six years, during which time she was a director and then deputy MD in the consumer practice.
Wray and Grierson were among the 14 new partners announced under Brady's changes. Other changes included removing the "irrelevant" distinction between corporate and consumer within the firm.
Freuds has announced a series of hires in recent months, including broadcaster Matt Barbet as a director; former Daily Mirror royal correspondent Victoria Murphy as an associate; Ogilvy PR managing partner Mark Schmid as a director; VCCP activation director planner Laura di Simone as digital channel planner; and Arif Haq, formerly of Contagious and Pepsi, as a partner.