Brain organoids derived from human induced pluripotent stem cells (hiPSC) recapitulate key features of the developing brain and can model complex neurological disorders. Integrating the PylRS/PylT pair into the genome of hiPSCs enables efficient site‐directed incorporation of non‐canonical amino acids (ncAAs) and allows derivatization of neurons and brain organoids with an expanded genetic code. The cover feature demonstrates how PylT recodes an amber stop codon within a GFP reporter to direct site‐specific incorporation of an ncAA, leading to GFP fluorescence throughout the organoid, as visible by light‐sheet microscopy. The method will help to implement existing ncAA‐based strategies for probing and manipulating proteins in hiPSC‐derived complex human disease models. More information can be found in the Full Paper by L. van Husen et al.