In this work, zeolite-containing microspherical composites based on kaolin were synthesized and modified with ammonium, lanthanum, and zirconium compounds to obtain active forms in the catalytic cracking reaction. The samples were studied using a number of physicochemical methods and tested in micro-pulse n-hexane cracking. Using scanning electron microscopy, it was found that the synthesized samples, in addition to the zeolite-containing composite, also contain a certain amount of pure zeolite phase, the largest in the La-containing samples. Differential scanning calorimetry showed that modification with La and Zr contributes to an increase in the thermal stability of the steamed forms of composites compared to the pure hydrogen form. In turn, the low-temperature nitrogen ad(de)sorption showed less destruction of the sample containing Zr during thermo-steam treatment. The observed effects were explained by the increase in the Si/Al ratio during steam treatment and Zr introduction, respectively. This is confirmed by a shift, in the IR spectra of the samples, of the absorption band corresponding to the asymmetric stretching vibrations of the T–O bonds of the framework tetrahedra after the appropriate modification procedures. The obtained composites were shown not to inferior to the industrial FCC catalyst from the former Engelhard Corp. in catalytic activity in the n-hexane cracking reaction, while they potentially are more resistant to coke formation after steam stabilization of their activity in the reactor/regenerator system. The best result was achieved when using zirconium due to the better diffusion characteristics of the Zr-containing catalyst and its higher resistance to thermal stress.