Generating graphs subject to strict structural constraints is a fundamental computational challenge in network science. Simultaneously preserving interacting properties-such as the diameter and the clustering coefficient- is particularly demanding. Simple constructive algorithms often fail to locate vanishingly small sets of feasible graphs, while traditional Markov-chain Monte Carlo (MCMC) samplers suffer from severe ergodicity breaking. In this paper, we propose a two-step hybrid framework combining Ant Colony Optimization (ACO) and MCMC sampling. First, we design a layered ACO heuristic to perform a guided global search, effectively locating valid graphs with prescribed diameter and clustering coefficient. Second, we use these ACO-designed graphs as structurally distinct seed states for an MCMC rewiring algorithm. We evaluate this framework across a wide range of graph edge densities and varying diameter-clustering-coefficient constraint regimes. Using the spectral distance of the normalized Laplacian to quantify structural diversity of the resulting graphs, our experiments reveal a sharp contrast between the methods. Standard MCMC samplers remain rigidly trapped in an isolated subset of feasible graphs around their initial seeds. Conversely, our hybrid ACO-MCMC approach successfully bridges disconnected configuration landscapes, generating a vastly richer and structurally diverse set of valid graphs.

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