The applications of spin-based quantum sensors to measurements probing fundamental physics are surveyed. Experimental methods and technologies developed for quantum information science have rapidly advanced in recent years, and these tools enable increasingly precise control and measurement of spin dynamics. Theories of beyond-the-Standard-Model physics predict, for example, symmetry violating electromagnetic moments aligned with particle spins, exotic spin-dependent forces, coupling of spins to ultralight bosonic dark matter fields, and changes to the local environment that affect spins. Spin-based quantum sensors can be used to search for these myriad phenomena, and offer a methodology for tests of fundamental physics that is complementary to particle colliders and large scale particle detectors. Areas of technological development that can significantly enhance the sensitivity of spin-based quantum sensors to new physics are highlighted.