This work presents a CAMD (computer-aided molecular design) approach for the design of working fluid mixtures used in ABR (absorption refrigeration) cycles. Compared to previous works, the proposed approach introduces two major improvements. It employs for the first time an ABR process model in the course of CAMD, hence enabling the evaluation of the generated mixtures considering process performance indicators. It enables for the first time the simultaneous generation and evaluation of molecular structures for both refrigerants and absorbents. The employed model and CAMD optimization problem formulation incorporates major ABR operational driving forces pertaining to efficient refrigeration, sufficient solubility of mixture components and ease of separation in the generator. The approach employs a multicriteria assessment methodology both during CAMD and for the evaluation of selected mixtures using a more rigorous ABR model at a second stage. The work identifies novel mixtures, with Acetaldehyde/2-Methoxyethyl acetate and Acetaldehyde/Methanediol exhibiting the highest performance. The latter exhibits 3% higher COP (coefficient of performance) and cooling output than the reference mixture NH3/H2O, whereas it operates at 87 and 89% lower high and low cycle pressures. The novel mixtures are also compared with novel mixtures previously identified through a heuristic approach by the authors. The latter mixtures indicate overall higher ABR performance but similar or worse performance in safety, health and environmental impact indices. Further performance improvements may be achieved by including into CAMD additional chemical groups to be able to simulate the complex absorbent structures available in published works.