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Moisture damage (MD) in bituminous mixtures occurs due to the loss of cohesion in the bitumen or adhesion between the binder and aggregates. The existence of moisture may influence the bonding between aggregates and bitumen, which may affect the moisture susceptibility of the bituminous mix. Therefore, there is a need to understand the bonding-debonding properties and the moisture susceptibility of binders and mixes, at the material selection stage. Surface free energy (SFE) method is one of the proven techniques to quantify the moisture susceptibility of bituminous mixtures, by using contact angle (CA) determination of the component materials of the mix. This study aimed to evaluate the effect of hydrated lime (HL) on the moisture susceptibility of bituminous mixtures, with control (VG30) bitumen and pyro-oil modified bitumen (POMB) having different percentages of pyro oil, using the SFE approach. Also, the study compared the SFE characteristics of VG30 and POMB with and without the optimum content of HL. POMB binders were prepared by the addition of high-density polyethylene (HDPE) pyro oil in percentages of 1, 3, and 5% in a control bitumen. HL was added as 20%, 25%, and 30% by weight of bitumen in VG30 and POMB bitumen. The aggregates used in the study were limestone, basalt, gravel, and their SFE components were directly considered from the literature. The sessile drop method was used to measure the CA of bitumen and, in turn, determine the various SFE parameters using Van Oss–Chaudhury–Good theory. The moisture susceptibility of mixtures with and without HL was evaluated and compared. From the results, the MD resistance of the bituminous mixtures with modified and unmodified bitumen was found to be increased after the optimum of HL, depending upon the type of aggregates used. Basalt has a 27.41%, 23.38%, and 10.48% greater energy ratio (ER) with POMB1/25, POMB3/25, and POMB5/30, respectively, than VG30/30, the highest ER in modified base bitumen. This indicates that HDPE pyro-oil treatment improves MD resistance for basalt. Whereas for limestone and gravel, VG30/30 gives a maximum value of ER as compared to any other combination of HL modified POMB. The ER values would assist highway agencies in selecting the most compatible binder–aggregate combinations. [ABSTRACT FROM AUTHOR]