We aimed to investigate the impact of surface roughness on liquid bridges between spherical particles. Sandblasting was used to control the particle size and produce glass beads and plates with different surface roughness. First, by measuring the advancing and receding contact angles of droplets on different rough surfaces, we analyzed the effects of surface roughness on wettability and hysteresis. Next, we used a custom-made liquid-bridge stretching device to measure the capillary forces of the liquid bridges between spherical particles with different surface roughness values. A charge-coupled device camera acquisition system was set up to capture the morphological changes of the liquid bridge during stretching, and Image View software was used to extract the morphological parameters of the liquid bridge. Theoretically, we reasonably simplified and solved the differential equations for the liquid bridge morphology and used the Young–Laplace equation to calculate the theoretical capillary force of the liquid bridge, providing an in-depth analysis of the influence of surface roughness on the capillary force. Finally, we studied the impact of surface roughness on the volume ratio of the liquid bridge during static stretching and the residual liquid remaining after the liquid bridge breaks. Experimental results indicated that, as the surface roughness increased, the hydrophobicity and wettability hysteresis of the solid surface also increased. The increased hydrophobicity of the surface reduces the solid-liquid contact area of the liquid bridges between the particles, making it easier to form “columnar” or “convex” liquid bridges. Additionally, the enhanced wettability hysteresis causes the solid-liquid contact boundary to lag during the stretching of the liquid bridge, resulting in a decrease in the solid-liquid contact angle. These factors directly alter the geometric shape of liquid bridges during static stretching, thereby affecting capillary forces. Meanwhile, the increase in surface roughness weakens the effect of gravity on the morphology of the liquid bridge, resulting in less liquid mass remaining on the lower sphere after the liquid bridge breaks as the surface becomes rougher.