Entanglement is a key resource for quantum computers, quantum-communication networks, and high-precision sensors. Macroscopic spin ensembles have been historically important in the development of quantum algorithms for these prospective technologies and remain strong candidates for implementing them today. This strength derives from their long-lived quantum coherence, strong signal, and ability to couple collectively to external degrees of freedom. Nonetheless, preparing ensembles of genuinely entangled spin states has required high magnetic fields and cryogenic temperatures or photochemical reactions. We demonstrate that entanglement can be realized in solid-state spin ensembles at ambient conditions. We use hybrid registers comprising of electron-nuclear spin pairs that are localized at color-center defects in a commercial SiC wafer. We optically initialize 103 identical registers in a 40-μm3 volume (with 0:95+0:05-0:07 fidelity) and deterministically prepare them into the maximally entangled Bell states (with 0.88 ± 0.07 fidelity). To verify entanglement, wedevelop a register-specific quantum-state tomography protocol. The entanglement of a macroscopic solid-state spin ensemble at ambient conditions represents an important step toward practical quantum technology.