Modern efforts to influence materials science with principles of biology have allowed fungal mycelial materials to take a foothold and develop novel solutions for the circular bioeconomy of tomorrow. However, recent studies have shown that the value of tomorrow’s green materials is not determined simply by their environmental viability, but rather by their ability to make the polluting materials of today obsolete. With an inherently strong structure of chitin and β-glucan, the ever-adaptable mycelia of fungi can compete at the highest levels with a litany of materials from leather to polyurethane foam to paper to wood. There are significant efforts to optimize pure mycelial materials (PMMs) through the entire process of species and strain selection, mycelial growth, and fabrication. Indeed, the promising investigations of novel species demonstrate how the diversity of fungi can be leveraged to create uniquely specialized materials. This review aims to highlight PMMs’ current trajectory, evaluate the successes in technology, and explore how these new materials can help shape a better tomorrow.