The field of materials for quantum information science is rapidly growing with a focus on scaling and integrating new solid-state qubits. However, despite the extraordinary progress, major challenges must still be overcome for scaling. Specifically, there is a critical need for efficient coupling of tens to hundreds of solid-state qubits and multiqubit error correction to mitigate environmental interactions. This Perspective looks forward to the challenges ahead in the realization of multiqubit operations and collective phenomena with a focus on solid-state quantum materials. We provide a theorists’ point of view on the modeling and rational design of these multiqubit systems. Our Perspective identifies a path for bridging the gap between the model Hamiltonians used to develop quantum algorithms and control sequences and the ab initio calculations used to understand and characterize single solid-state-based qubits.