This thesis presents work on a holistic approach for improving the overall design of solar cooling systems driven by solar thermal collectors. Newly developed methods for thermodynamic optimization of hydraulics and control were used to redesign an existing pilot plant. Measurements taken from the newly developed system show an 81% increase of the Solar Cooling Efficiency (SCEth) factor compared to the original pilot system. In addition to the improvements in system design, new efficiency factors for benchmarking solar cooling systems are presented. The Solar Supply Efficiency (SSEth) factor provides a means of quantifying the quality of solar thermal charging systems relative to the usable heat to drive the sorption process. The product of the SSEth with the already established COPth of the chiller, leads to the SCEth factor which, for the first time, provides a clear and concise benchmarking method for the overall design of solar cooling systems. Furthermore, the definition of a coefficient of performance, including irreversibilities from energy conversion (COPcon), enables a direct comparison of compression and sorption chiller technology. This new performance metric is applicable to all low-temperature heat-supply machines for direct comparison of different types or technologies. The achieved findings of this work led to an optimized generic design for solar cooling systems, which was successfully transferred to the market.