This paper first addresses the definition of various objectives involved in eco-efficient processes, taking simultaneously into account ecological and economic considerations. The environmental aspect at the preliminary design phase of chemical processes is quantified by using a set of metrics or indicators following the guidelines of sustainability concepts proposed by IChemE (2001). The resulting multiobjective problem is solved by a genetic algorithm following an improved variant of the so-called NSGA II algorithm. A key point for evaluating environmental burdens is the use of the package ARIANE (TM), a decision support tool dedicated to the management of plants utilities (steam, electricity, hot water, etc.) and pollutants (CO(2), SO(2), NO, etc.), implemented here both to compute the primary energy requirements of the process and to quantify its pollutant emissions. The well-known benchmark process for hydrodealkylation (HDA) of toluene to produce benzene, revisited here in a multiobjective optimization way, is used to illustrate the approach for finding eco-friendly and cost-effective designs. Preliminary biobjective studies are carried out for eliminating redundant environmental objectives. The trade-off between economic and environmental objectives is illustrated through Pareto curves. In order to aid decision making among the various alternatives that can be generated after this step, a synthetic evaluation method, based on the so-called Technique for Order Preference by Similarity to Ideal Solution (TOPSIS) (Opricovic & Tzeng, 2004), has been first used. Another simple procedure named FUCA has also been implemented and shown its efficiency vs. TOPSIS. Two scenarios are studied; in the former, the goal is to find the best trade-off between economic and ecological aspects while the latter case aims at defining the best compromise between economic and more strict environmental impacts. (C) 2011 Elsevier Ltd. All rights reserved.