Graduate student staff (GSS) positions, commonly used in centers for teaching and learning (CTL) to expand capacity and extend disciplinary connections on campus, also offer the potential for a meaningful developmental experience for the students who fill them. Drawing on the literature on graduate student mentorship, we lay out goals and aligned practices to inform the mentoring of GSS in CTL aimed at advancing their pedagogical, professional, and personal development. Such deliberate attention to mentoring in a CTL context can enhance the experience and development of the GSS themselves, as well as improve the work of the CTL.