We probe resonant dipolar interactions between ultracold ${}^{40}\mathrm{K}{}^{87}\mathrm{Rb}$ molecules and Rydberg ${}^{87}\mathrm{Rb}$ atoms in an optically trapped ensemble. Through state-selective ionization detection of the KRb molecules, we observe resonant energy transfer at 2.227 GHz from Rydberg atoms to molecules under a tunable external electric field. We measure a broadening up to 3.5 MHz, for the Rb Rydberg excitation spectrum, which matches a Monte Carlo simulation that describes a Rydberg atom and neighboring molecules evolving under a dipole-dipole interacting Hamiltonian. The demonstrated interspecies dipolar interaction is a key ingredient for hybrid Rydberg-polar molecule systems, where the advantages of each system can be leveraged and combined.

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• Dipolar Rydberg atoms
• Dipolar molecules
• Electric dipole-dipole interactions
• Mixtures of atomic and/or molecular quantum gases