The ability to detect and identify molecules at high sensitivity without the use of labels or capture agents is important for medical diagnostics, threat identification, environmental monitoring, and basic science. Microtoroid optical resonators, when combined with noise reduction techniques, have been shown capable of label-free single molecule detection; however, they still require a capture agent and prior knowledge of the target molecule. Optical frequency combs can potentially provide high precision spectroscopic information on molecules within the evanescent field of the microresonator; however, this has not yet been demonstrated in air or aqueous biological sensing. For aqueous solutions in particular, impediments include coupling and thermal instabilities, reduced Q factor, and changes to the mode spectrum. Here we overcome a key challenge toward single-molecule spectroscopy using optical microresonators: the generation of a frequency comb at visible to near-IR wavelengths when immersed in either air or aqueous solution. The required dispersion is achieved via intermodal coupling, which we show is attainable using larger microtoroids, but with the same shape and material that has previously been shown ideal for ultra-high sensitivity biosensing. We believe that the continuous evolution of this platform will allow us in the future to simultaneously detect and identify single molecules in both gas and liquid at any wavelength without the use of labels.