Substitution of Ru(II)‐based chromophores with cheaper Cr(III)‐ based complexes in optically active metallo‐supramolecular architectures is limited by the lack of synthetic strategies leading to heteroleptic Cr(III)‐polypyridyl complexes with long excitedstate lifetimes. Herein, we report on a versatile method yielding heteroleptic bis(terdentate) Cr(III) complexes with room temperature millisecond range excited‐state lifetimes, tuneable electronic and photophysical properties and easy anchoring possibilities.