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Urban land optimization in urban agglomerations plays an important role in promoting territorial spatial planning to achieve high-quality development, land ecological suitability (LES) is one of the important variables influencing its urbanization and needs to be considered in urban growth simulation and modeling. This research proposed a multi-objective urban land optimization (MULO) model based on the non-dominated sorting genetic algorithm II (NSGA-II) which integrates the LES assessment. MULO starts with LES analysis based on a fuzzy analytical hierarchy process (AHP) and a minimum cumulative resistance (MCR) model. Then, two-step linear regression is used to optimize the quantity structure of built-up land. Finally, suitability and compactness are assigned to NSGA-II as objectives to obtain optimal spatial patterns. Taking the example of the Guangdong–Hong Kong–Macao Greater Bay Area, we found that all the newly added built-up land in 2030 is distributed in peri-urban areas around the original settlements, with approximate clustering in the northern part of Guangzhou and the southern part of Foshan under a balanced development scenario. This study highlights the importance of LES in urban growth modeling, and MULO can provide effective support for the spatial planning of urban agglomerations.