Mapping intratumoral heterogeneity such as vasculature and margins is important during intraoperative applications. Desorption electrospray ionization mass spectrometry (DESI-MS) has demonstrated potential for intraoperative
tumor imaging using validated MS profiles. The clinical translation of DESI-MS into a universal label-free imaging technique thus requires access to MS profiles characteristic to
tumors and healthy tissues. Here, we developed
contrast agent mass spectrometry imaging (CA-MSI) that utilizes a magnetic resonance imaging (MRI)
contrast agent targeted to disease sites, as a label, to reveal
tumor heterogeneity in the absence of known MS profiles. Human
breast cancer tumors grown in mice were subjected to CA-MSI using
Gadoteridol revealing
tumor margins and vasculature from the localization of [Gadoteridol+K](+) and [Gadoteridol+Na](+) adducts, respectively. The localization of the [Gadoteridol+K](+) adduct as revealed through DESI-MS complements the in vivo MRI results. DESI-MS imaging is therefore possible for
tumors for which no characteristic MS profiles are established. Further DESI-MS imaging of the flux of the
contrast agent through mouse kidneys was performed indicating secretion of the intact label.