Harnessing entanglement and quantum coherence plays a central role in advancing quantum technologies. In quantum optical light-atom platforms, these two fundamental resources are often associated with a Jaynes-Cummings model description describing the coherent exchange of a photon between an optical resonator mode and a two-level spin. In a generic nonlinear spin-boson system, more photons and more modes will take part in the interactions. Here we consider such a generalization: the two-mode multiphoton Jaynes-Cummings (MPJC) model. We demonstrate how entanglement and quantum coherence can be optimally generated and subsequently manipulated in experimentally accessible parameter regimes. A detailed comparative analysis of this model reveals that nonlinearities within the MPJC interactions produce genuinely non-Gaussian entanglement, devoid of Gaussian contributions, from noisy resources. More specifically, strong coherent sources may be replaced by weaker, incoherent ones, significantly reducing the resource overhead, though at the expense of reduced efficiency. At the same time, increasing the multiphoton order of the MPJC interactions expedites the entanglement generation process, thus rendering the whole generation scheme again more efficient and robust. We further explore the use of additional dispersive spin-boson interactions and Kerr nonlinearities in order to create spin coherence solely from incoherent sources and to enhance the quantum correlations, respectively. As for the latter, somewhat unexpectedly, there is not necessarily an increase in quantum correlations due to the augmented nonlinearity. Towards possible applications of the MPJC model, we show how, with appropriately chosen experimental parameters, we can engineer arbitrary NOON states as well as the tripartite W state. Published by the American Physical Society 2024