Taking advantage of quantum mechanics for executing computational tasks faster than classical computers1 or performing measurements with precision exceeding the classical limit2,3 requires the generation of specific large and complex quantum states. In this context, cluster states4 are particularly interesting because they can enable the realization of universal quantum computers by means of a ‘one-way’ scheme5, where processing is performed through measurements6. The generation of cluster states based on sub-systems that have more than two dimensions, d-level cluster states, provides increased quantum resources while keeping the number of parties constant7, and also enables novel algorithms8. Here, we experimentally realize, characterize and test the noise sensitivity of three-level, four-partite cluster states formed by two photons in the time9 and frequency10 domain, confirming genuine multi-partite entanglement with higher noise robustness compared to conventional two-level cluster states6,11–13. We perform proof-of-concept high-dimensional one-way quantum operations, where the cluster states are transformed into orthogonal, maximally entangled d-level two-partite states by means of projection measurements. Our scalable approach is based on integrated photonic chips9,10 and optical fibre communication components, thus achieving new and deterministic functionalities. The creation and manipulation of large quantum states is necessary for quantum information processing tasks. Three-level, four-partite cluster states have now been created in the time and frequency domain of two photons on-chip.