In this paper, an Ising model with hybrid spins was used to construct the edge-modified kekulene multilayer cluster. Using Monte Carlo simulation, the magnetic properties of the edge-modified kekulene multilayer cluster were studied. The variations of several physical quantities with temperature field and external magnetic field are discussed, such as magnetization, magnetic susceptibility, energy, and hysteresis loop. The analysis revealed that the saturation magnetization values of the whole system induced by the crystal field D-a are more abundant than that induced by the crystal field D-b. The results of phase diagrams of T-b illustrate that decreasing crystal field |D-b| and increasing exchange coupling J(b) can improve the blocking temperature T-b, but T-b is not sensitive to the change of the crystal field |D-a| and exchange coupling |J(ab)|. Some multi-loop hysteresis characteristics including double-loop, triple-loop, quadruple-loop, and sextuple-loop hysteresis behaviors could be exhibited under the influence of diverse parameters.