Given the importance of preserving the mechanical properties of recycled isotactic polypropylene (iPP) during its processing, this work provides an improved understanding of the contribution of introducing physical or chemical crosslinks using the dissipative particle dynamics (DPD) method, which makes it possible to model iPP structures with a realistic range of crosslink densities. First, the protocol to build a coarse‐grained model of iPP from an all‐atom expression by Bayesian optimization is described. A Bayesian optimization procedure employing two different cutoff distances successfully provides optimal DPD parameters reproducing iPP's properties compared to the all‐atom system. Then, the coarse‐grained iPP model with optimal DPD parameters is applied to study structures containing a realistic range of crosslink densities to evaluate their mechanical properties. These calculations demonstrate that the mechanical properties such as the Young's modulus and ultimate strength increase while the fracture strain decreases with an increase in the crosslink density, which is consistent with experimental observations. The results also show that there is a critical crosslink density above which these properties start to be improved due to the introduction of crosslinks. These findings can help us to obtain targeted properties of recycled iPP by introducing physical or chemical crosslinks.