In this study, graphene oxide (GO) was prepared using the improved Hummers’ method, and GO was carboxylated and modified into hydroxylated graphene oxide (GOH). Diatomaceous earth (DE), which exhibits stable chemical properties, a large specific surface area, and high porosity, as well as chitosan/magnetic chitosan, was loaded by solution blending. Subsequently, carboxylated graphene oxide/diatomite/chitosan (GOH/DCS) and carboxylated graphene oxide/diatomite/magnetic chitosan (GOH/DMCS) composites were prepared through simple solid–liquid separation. The results showed that the modified GOH/DCS and GOH/DMCS composites could be used to remove lanthanum La(III)), which is a rare earth element. Different factors, such as initial solution concentration, pH of the solution, adsorbent dosage, adsorption contact time, and adsorption reaction temperature, on adsorption, were studied, and the adsorption mechanism was explored. An adsorption–desorption recycling experiment was also used to evaluate the recycling performance of the composite material. The results show that at the initial solution concentration of 50 mg·g−1, pH = 8.0, 3 g·L−1 adsorbent dosage, reaction temperature of 45 °C, and adsorption time of 50 min, the adsorption effect is the best. The adsorption process is more in line with the pseudo-second-order kinetic model and Langmuir model, and the internal diffusion is not the only controlling effect. The adsorption process is an endothermic and spontaneous chemical adsorption process. The maximum adsorption capacity of GOH/DMCS for La(III) at 308K is 302.51 mg/g through model simulation. After four adsorption–desorption cycles, the adsorption capacity of the GOH/DMCS composite for La(III) initially exceeded 74%. So, GOH/DMCS can be used as a reusable and efficient adsorbent.