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In this paper we derive for the first time the complete gravitational quartic-in-spin interaction of generic compact binaries at the next-to-leading order in the post-Newtonian (PN) expansion. The derivation builds on the effective field theory for gravitating spinning objects, and its recent extensions, in which new type of worldline couplings should be considered, as well as on the extension of the effective action of a spinning particle to quadratic order in the curvature. The latter extension entails a new Wilson coefficient that appears in this sector. This work pushes the precision frontier with spins at the fifth PN (5PN) order for maximally-spinning compact objects, and at the same time informs us of the gravitational Compton scattering with higher spins. [ABSTRACT FROM AUTHOR]