<p>Correlations between neuronal excitability and synaptic coupling are biologically motivated yet remain underexplored in theoretical models. Here, intrinsic excitability denotes a neuron-specific propensity to spike, whereas excitatory and inhibitory effects refer to the sign of the coupling-mediated network input. Within this framework, we show that embedding such structured correlations in a network of Theta neurons, analyzed through the Ott–Antonsen reduction, induces multi-window bistability, state-dependent clustering along the excitability axis, and distinct routes to chaos. Localized suppressive effects can arise without imposing a fixed excitatory/inhibitory population partition, as the excitability-dependent coupling profile can encode either reductions of positive network drive or genuine effective inhibitory interactions. These results suggest that correlation geometry can serve as a compact organizing variable linking microstructural diversity to emergent dynamical complexity in large-scale excitable systems, with possible implications for understanding structure-function relationships beyond neural circuits.</p>