In this paper, we explore the interactions between light axion-like particles (ALPs) and top quarks, gluons, and W-bosons. Utilizing high-energy probes at the LHC, we probe these couplings in the context of single top quark production associated with a W-boson and an ALP. We analyze the latest LHC Run II data on tt spin correlation measurements to establish constraints on these couplings. Additionally, we compare these constraints with those derived from loop-induced couplings and indirect searches involving B-meson decays. Furthermore, we derive two-dimensional limits on the ALP couplings with top quarks and gluons.