Chemotherapeutic-loaded bone cement may be an effective method of drug delivery for the management of cancer-related vertebral fractures that require cement injection for pain relief. Recent advancements in the development of aluminum-free glass ionomer cements (GICs) have rendered this class of biomaterials clinically viable for such applications. To expand the therapeutic benefits of these materials, this study examined, for the first time, their drug delivery potential. Through incrementally loading the GIC with methotrexate (MTX) by up to 10-wt%, composition-property relationships were established, correlating MTX loading with working time and setting time, as well as compressive strength, drug release, and cytotoxic effect over 31 days. The most significant finding of this study was that MTX was readily released from the GIC, while maintaining cytotoxic activity. Release correlated linearly with initial loading and appeared to be diffusion mediated, delivering a total of 1-2% of the incorporated drug. MTX loading in this range exerted minimal effects to handling and strength, indicating the clinical utility of the material was not compromised by MTX loading. The MTX-GIC systems examined herein are promising materials for combined structural delivery applications.