In this work, we describe a reproducible method to prepare polymeric colloidal nanospheres of poly(ethyl-2-cyanoacrylate), poly(butylcyanoacrylate), poly(hexylcyanoacrylate) and poly(octylcyanoacrylate) with a magnetite core, and loaded with the anticancer drug Tegafur. The method is based on the emulsion polymerization procedure, often used in the synthesis of poly(alkylcyanoacrylate) nanospheres for drug delivery. The heterogeneous structure of the particles confer them both magnetic-field responsiveness and potential applicability as drug carriers. In order to investigate to what extent is this target achieved, we compare the surface electrical properties of the core/shell particles with those of both the nucleus and the coating material. The hysteresis cycles of both magnetite and composite particles demonstrate that the polymer shell reduces the magnetic responsiveness of the particles, but keeps their soft ferrimagnetic character unchanged. A detailed investigation of the capabilities of the core/shell particles to load this drug is shown. We found, by means of spectrophotometric and electrophoretic measurements, the existence of two drug loading mechanisms: absorption or entrapment in the polymeric network, and surface adsorption. The type of polymer, the pH and the drug concentration are the main factors determining the drug incorporation to the nanoparticles. The release studies showed a biphasic profile affected by the type of polymeric shell, the type of drug incorporation and the amount of drug loaded.