We compute, up to 4th post-Newtonian (4PN) order, the gauge-invariant stability criterion determining the innermost stable circular orbit (ISCO) for arbitrary-mass compact binaries with spins aligned with the orbital angular momentum. Our calculation, a perturbation analysis, incorporates spin-orbit and spin-spin contributions, both up to next-to-next-to-leading order, as well as leading-order cubic and quartic spin contributions, all calculated in prior works within the effective-field-theory (EFT) Hamiltonian formalism. In the test-mass limit, we recover the Kerr ISCO truncated at 4PN order. Estimating the ISCO shift at first order in the mass ratio and comparing our results with numerical gravitational self-force (GSF) calculations, we find good agreement for retrograde spin (the smallest discrepancy being obtained for maximal retrograde spin) and moderate prograde spin. For nearly maximal prograde spin, the PN approach fails to determine the ISCO, for it is close to the black hole (BH) horizon. We also estimate the ISCO shift due to the test-particle spin and compare our result with the exact prediction from the Mathisson-Papapetrou-Dixon (MPD) equations for a spinning particle orbiting a Kerr BH. Finally, we discuss the stability and the ISCO of corotating BH binaries.