Hardware functional verification relies on high-quality assertions to expose design bugs and establish confidence in Register Transfer Level (RTL) designs. Yet existing assertion mining methods still struggle to produce complete and reliable assertion sets. Random or limited traces fail to cover hard-to-reach behaviors, and one-shot generation provides little feedback about what remains unverified or how the assertion set should be improved. As a result, critical design behaviors can remain uncovered even when many assertions are generated. We present NeuroAssertion, a coverage-driven assertion generation framework that combines formal trace generation, syntax-guided synthesis (SyGuS), and an agent-inspired refinement process within a unified framework. Our framework first converts hard-to-reach control-flow conditions into formal reachability objectives, uses model checking to generate behaviorally diverse traces, and mines initial assertions from these traces with SyGuS. It then performs targeted agent-inspired refinement under verification feedback. One LLM first proposes candidate assertions for uncovered regions, and if a candidate fails formal checking, a second LLM generates a repair grammar that guides constrained symbolic synthesis in a neuro-symbolic repair procedure. Experimental results show that this framework delivers around 2x more assertions and about 2x higher mutation coverage than traditional assertion mining methods.