<p>Taita Hills are one of the most important biodiversity hotspots of Kenya but are experiencing a high rate of deforestation due to the to the conversion of its original forestland to agriculture and settlement during the last century. These landscape dynamics, coupled with rainfall fluctuations in these critical ecosystems, may significantly affect water resource distribution and food security in Taita Taveta County and its environs. This study aimed to establish the trends of land use/cover change (LUCC) in the Wundanyi catchment from 1970 to 2030 and predict their specific and combined effects on surface runoff and stream flow in the same period. The analysis was based on statistical trend analysis and dynamic landscape modeling using both historical and primary data from the Wundanyi catchment and Landsat TM and ETM+ imagery of Taita Hills for 1990, 2000, and 2010. Results show highly variable mean seasonal and annual values of discharge in Wundanyi catchment, probably attributed to environmental changes affecting Taita Hills in general and Wundanyi catchment in particular. Compared to 1990, major land use/cover changes in 2010 were featured by the expansion of built-up area (250%), plantation forest (23.7%), broadleaved forest (17.4%), and thicket (15.9%). It was also notable the decrease in woodland (−30.3%), cropland (−21.6%), and shrubland (−0.8%). Dynamic spatial trends by the year 2030 will be evidenced by increased thicket by 0.41% per annum (<em>R</em><sup>2</sup> = 81.6%) and by decreased plantation forests (−0.13%; <em>R</em><sup>2</sup> = 91.3%), woodland (−0.10%; <em>R</em><sup>2</sup> = 77.6%), shrubland (−0.11%; <em>R</em><sup>2</sup> = 85.2%), broadleaved forests (−0.03%; <em>R</em><sup>2</sup> = 56.6%) and cropland (−0.09%; <em>R</em><sup>2</sup> of 84.4). These changes will shape the catchment landscape and influence its hydrology, unless the existing forest and agricultural policy interventions are enforced. Hence, crop diversification, agroforestry, and soil and water conservation structures are recommended to maintain effective control of LUCC on hydrological processes going on in the Wundanyi catchment.</p>