Despite the rampant discovery of tunable magnetic properties using magnetoâionic gating, e.g., magnetic anisotropy, exchange bias, and exchange interactions, there are few studies that give a quantitative understanding of the reversible and irreversible effects of ionic infiltration. In this study, in situ vibrating sample magnetometry, superconducting quantum interference device magnetometry, and Xâray magnetic circular dichroism (XMCD) reveal the reversible and irreversible control of magnetization, anisotropy, proximityâeffects, spin, and orbital angular momenta. Pd/Co/Pd trilayers, loaded using solidâstate hydrogenâion gating, show a decrease in the saturation magnetization of Co, and an increase in the proximityâinduced moment of Pd. This results in little to no change in the net effective magnetization, yet, allows for the effective anisotropy to be reversibly controlled by 270 kJ mâ3. The reversible control of the effective anisotropy is dominated by a reversible change in surface anisotropy, however, under repeated cycling, irreversible evolution occurs in the heterostructure. XMCD measurements indicate this is partly due to hydrogenâinduced modification of the spin and orbital angular momenta. Together, these measurements indicate that the origin of the reversible and irreversible effects of magnetoâionic gating is interfacial and provides crucial insight to scale and optimize thin film heterostructures for enhanced longevity and faster response time.