Magnetic nanoarchitectures have been used to introduce multifunctionality in biopolymeric matrices. Bionanocomposite foams based on the corn protein zein were prepared for the first time using the hydrophobic properties of zein in a sequential treatment consisting of the removal of ethanol-soluble fractions, followed by the water swelling of the remaining phase and a further freeze-drying process. When this protocol is applied to zein pellets, they can be consolidated as porous monoliths. Moreover, it is possible to incorporate diverse types of inorganic nanoparticles in the starting pellet to produce the bionanocomposite foams. In particular, the preparation of superparamagnetic foams has been explored using two approaches: the direct incorporation of magnetite nanoparticles in a ferrofluid by impregnation in the foams, and the application of the foaming process to mixtures of zein with magnetite nanoparticles alone or previously assembled into sepiolite clay fibers. The first methodology leads to the production of inhomogeneous foams, while the use of magnetite nanoparticles and better Fe3O4-sepiolite nanoarchitectured materials as fillers results in more homogeneous materials with improved water stability and mechanical properties, offering superparamagnetic behavior. The resulting multifunctional foams have been tested in adsorption processes using the herbicide 4-chloro-2-methylphenoxyacetic acid as a model pollutant, confirming their potential utility in decontamination applications in open waters as they can be easily recovered from the aqueous medium using a magnet.