The study aimed to analyze the effect of the addition of nano-hydroxyapatite (nano-HA) particles on the mechanical properties of experimental adhesive (EA). Furthermore, dentin interaction of EA (without nano-HA) and EA with nano-HA (hereon referred to as HA-10%) were also investigated and equated. Methods consisting of scanning electron microscopy (SEM)–energy-dispersive X-ray spectroscopy (EDX), micro-Raman spectroscopy, micro-tensile bond strength (µTBS) test, and Fourier transform infrared (FTIR) spectroscopy were employed to study nano-HA particles shape, dentin bond strength, degree of conversion (DC), and adhesive–dentin interaction. Ninety teeth (N = 90) were collected, and pre-bonding, conditioning of dentin was performed utilizing phosphoric acid (H3PO4) etching, photodynamic therapy (PDT), and ER-CR-YSGG (ECY) laser. The teeth were set to form bonded specimens using two adhesives. Nano-HA particles were spherical-shaped, and EDX confirmed the presence of oxygen, calcium, and phosphorus. Micro-Raman spectroscopy revealed distinct phosphate and carbonate peaks for nano-HA. The µTBS test demonstrated highest values for HA-10% group on the H3PO4 conditioned dentin. The greatest DC was observed for the EA group. The addition of nano-HA-10 wt.% particles in dentin adhesive resulted in improved bond strength. The incorporation also demonstrated acceptable DC (although lower than EA group), suitable dentin interaction, and resin tag formation.