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Complex chalcogenides in the MPS3 family of materials (M = Mn, Fe, Co, and Ni) display remarkably different phase progressions depending upon the metal center orbital filling, character of the P–P linkage, and size of the van der Waals gap. There is also a stacking pattern and spin state difference between the "lighter" and "heavier" transition metal-containing systems that places CoPS3 at the nexus of these activities - even though this compound is under-explored from a properties point of view. Here, we bring together Raman scattering and infrared absorption spectroscopies with x-ray techniques to identify a structural aspect to the 119 K magnetic ordering transition as well as a remarkable lower temperature set of magnon-phonon pairs that engage in avoided crossings along with a magnetic scattering continuum that correlates with phonon lifetime effects. These findings point to strong spin-phonon entanglement as well as opportunities to control these effects under external stimuli.