Thiourea-formaldehyde (TF) resin is prepared by polycondensation of its two precursors; the incorporation of pre-formed magnetite particles allows synthesizing a magnetic derivative of TF (MTF). These materials are applied to the sorption of two dyes (titan yellow, TY, and rose bengal, RB). Ultrasonic treatment (UT) is tested as an alternative to mechanical agitation (MA). The two sorbents are characterized by scanning electron microscopy, vibrating-sample magnetometry, BET surface area analysis, thermogravimetric analysis, Fourier-transform infrared and NMR spectroscopy, zetametry. Sorption properties are compared for TF and MTF under both MA and UT; considering pH effect, uptake kinetics (modeled using the pseudo-second order rate equation, and resistance to intraparticle diffusion), sorption isotherms (fitted by the Langmuir and Sips equations), the effect of competitor ions, and the desorption efficiency. Optimum sorption occurs at pH 3 (balance between (a) the electrostatic interactions between protonated groups (sorbent) and anionic forms of the dyes, and (b) the competitor effects of counter anions). UT strongly decreases the contact time required for reaching equilibrium (from 240 min to 30 min). UT increases the sorption capacities: in the range 0.3–0.6 mmol dye g−1 (MA) up to 0.9–1 mmol dye g−1. The magnetic core does not change kinetics, while it increases TF sorption capacities for both TY and RB. Under UT, the maximum sorption capacities are comparable for TF and MTF; however, the affinity of MTF remains higher than TF for the two dyes. Alkaline NaCl solutions completely desorb the dyes; UT decreases both the contact time and the NaCl concentration required for achieving the complete desorption of loaded dyes. The sorbents are recycled with high stability in sorption performance for at least five cycles.