With the advancement of rare-earth luminescent materials, developing composites with tunable luminescent properties poses a significant challenge. In this study, we synthesized HALs@YF3:Eu3+ scintillator material that emits red light by utilizing halloysites (HALs) as base materials and then surface modified with europium-doped YF3 via hydrothermal synthesis. The yielded product HALs@YF3:Eu3+ was characterized by TEM, SEM, XRD, and XPS, and then incorporated into the epoxy resin to endow X-ray scintillating abilities in the obtained composite with enhanced mechanical properties. Moreover, the green-emitting scintillator was also incorporated into the epoxy resin along with HALs@YF3:Eu3+ with varying feed ratios to afford the epoxy resin composites with tunable emission behaviors from red to green. This study demonstrates a valuable approach for applying epoxy resin composite materials in the field of radioluminescence.