A waterfall highlights the locus of active fluvial erosion of bedrock, and its mechanism has been the subject of several studies; however, erosional processes remain to be clarified for specific rock structures composing a waterfall. Herein, the detailed morphology of cliffs around a waterfall is examined by a terrestrial laser scanning (TLS) approach to analyze erosional processes occurring in the cliffs. The study site is Kegon Falls in Japan, which has a vertical drop of surface water from the top of its cliff and groundwater outflows from its lower portion. The entire cliff is mostly overhanging and minor rockfalls are often observed. The latest major rockfall occurred in 1986, causing an approximate 8-m upstream shift of the waterfall lip. From the point cloud obtained by TLS measurement, a digital elevation model on a vertical plane was generated, and cross-sectional profiles were extracted. A distinct 5- to 10-m depression was found at the bottom of the upper andesite layer of the waterfall cliff, which appears to have been formed by freeze-thaw and wet-dry weathering following the upstream shift of the surface water drop. Stability analysis of the waterfall cliff with an undercutting notch indicates that the igneous rock composing the cliff is sufficiently strong to maintain its current overhanging shape and that catastrophic collapse of the entire waterfall face rarely occurs. Following the formation of the depression, the upper cliff face appears to have been gradually eroded by gravitational collapses of relatively small blocks bounded by columnar and platy joints.