A method for the versatile synthesis of novel, mussel-inspired, electrospun nanofibers with catechol moieties is reported. These mussel-inspired nanofibers are used to bind iron oxide nanoparticles (IONPs) and the borate-containing anticancer drug Bortezomib (BTZ) through a catechol metal binding mechanism adapted from nature. These smart nanofibers exhibit a unique conjugation of Bortezomib to their 1, 2-benzenediol (catechol) moieties for enabling a pH-dependent drug delivery towards the cancer cells and the IONPs via strong coordination bonds for exploiting the repeated application of hyperthermia. Thus the synergistic anticancer effect of these mussel-inspired magnetic nanofibers were tested in vitro for the repeated application of hyperthermia along with the chemotherapy and found that the drug-bound catecholic magnetic nanofibers exhibited excellent therapeutic efficacy for potential anticancer treatment.