Photonic quantum technology increasingly uses frequency encoding to enable higher quantum information density and noise resilience. Pulsed time-frequency modes (TFM) represent a unique class of spectrally encoded quantum states of light that enable a complete framework for quantum information processing. Here, we demonstrate a technique for direct generation of entangled TFM-encoded states in single-pass, tailored down-conversion processes. We achieve unprecedented quality in state generation-high rates, heralding efficiency, and state fidelity-as characterized via highly resolved time-of-flight fiber spectroscopy and two-photon interference. We employ this technique in a four-photon entanglement swapping scheme as a primitive for TFM-encoded quantum protocols.