The invention provides a preparation method of modified mussel shells. The preparation method comprises the following steps: S1, preparing magnetic nanoparticles; S2, carrying out pretreatment of mussel shells; S3, preparing magnetic mussel shells: wherein respectively adding the magnetic nanoparticles and ammonia water into deionized water, heating to a reaction temperature, dropwise adding a silane coupling agent, adding mussel shell powder, reacting, cooling to room temperature, and carrying out magnet separation for later use; and S4, preparing the modified mussel shells: wherein adding lactic acid, a silane coupling agent and the magnetic mussel shells into deionized water, uniformly stirring, slowly dropwise adding a catalyst solution, stirring and reacting at room temperature, washing an obtained product with the deionized water and absolute ethyl alcohol for three times respectively, magnetically separating, drying and grinding to obtain the modified mussel shells. The modifiedmussel shells have good adsorption performance on methylene blue, modification conditions are simple, operation is convenient, and high operability is achieved. The waste mussel shells are used as raw materials, so that the method has good environmental benefits and can generate better economic benefits.