In order to accurately evaluate the adhesion of asphalt modified with natural asphalt and aggregate, the contact angles of three liquids on the sample surface of asphalt modified with natural asphalt were measured based on sessile drop method. According to the theory of surface physical chemistry, the measuring method of polar component and dispersion component for asphalt surface free energy under the condition of room temperature was determined. The surface free energies of base asphalt and asphalts modified with different dosages of natural asphalt were calculated. The relationship between asphalt surface free energy and asphalt-aggregate adhesion grade was analyzed based on the test result by using water-boiling method. Test result shows that the surface free energies of 70# grade A base asphalt and asphalt modified with 8% natural asphalt are 10.60,18.60 mJ·m-2 respectively, so the surface free energy of asphalt modified with natural asphalt increases distinctly with the addition of natural asphalt. There is a good correlation between asphalt-aggregate adhesion and the surface free energy of asphalt calculated by contact angle method. The natural asphalt contains higher polar functional groups such as O, S and N etc. High contents of asphaltene and net structure can absorb the light components of base asphalt such as saturates, aromatics. The increase of surface free energy for asphalt modified with natural asphalt is attributed to the polar functional groups and the absorbing functions. 4 tabs, 4 figs, 23 refs. ©, 2015, Chang'an University. All right reserved.