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Quantum information carriers with higher dimension than the canonical qubit offer significant advantages. However, manipulating such systems is extremely difficult. We show how measurement-induced nonlinearities can dramatically extend the range of possible transforms on biphotonic qutrits—<?format ?>three-level quantum systems formed by the polarization of two photons in the same spatiotemporal mode. We fully characterize the biphoton-photon entanglement that underpins our technique, thereby realizing the first instance of qubit-qutrit entanglement. We discuss an extension of our technique to generate qutrit-qutrit entanglement and to manipulate any bosonic encoding of quantum information.