In order to design new nanomaterials with improved functionalities, magnetite nanoparticles (MNP) modified with arylazopyrazole (AAP) molecular photoswitches are presented. Water dispersibility is achieved by using poly(acrylic acid) (pAA) as a multidentate ligand, which is modified with AAP by amide coupling. The polymer ligand stabilizes the MNP, allows for E-Z isomerization of the photoswitch, and provides pH responsiveness. Three different AAP are synthesized and attached to pAA via amide coupling giving pAA-AAP with photoswitches substituted statistically along the hydrophilic polymer backbone. MNP are synthesized by coprecipitation and pAA-AAP is introduced as a stabilizing agent in situ. Photoisomerization of pAA-AAP and pAA-AAP@MNP is investigated showing good photostationary states and cyclability. The MNP can be assembled and dispersed reversibly in water either by applying a magnetic field or by a change in pH.