Novel low‐power adiabatic sequences are demonstrated for in vivo localized two‐dimensional correlated MR spectroscopy, such as correlated spectroscopy and total correlated spectroscopy. The design is based on three new elements for in vivo two‐dimensional MRS: the use of gradient modulated constant adiabaticity GOIA‐W(16,4) pulses for (i) localization (correlated spectroscopy and total correlated spectroscopy) and (ii) mixing (total correlated spectroscopy), and (iii) the use of longitudinal mixing (z‐filter) for magnetization transfer during total correlated spectroscopy. GOIA‐W(16,4) provides accurate signal localization, and more importantly, lowers the SAR for both total correlated spectroscopy mixing and localization. Longitudinal mixing improves considerably (fivefolds) the efficiency of total correlated spectroscopy transfer. These are markedly different from previous 1D editing total correlated spectroscopy sequences using spatially nonselective pulses and transverse mixing. Fully adiabatic (adiabatic mixing with adiabatic localization) and semiadiabatic (adiabatic mixing with nonadiabatic localization) methods for two‐dimensional total correlated spectroscopy are compared. Results are presented for simulations, phantoms, and in vivo two‐dimensional spectra from healthy volunteers and patients with brain tumors obtained on 3T clinical platforms equipped with standard hardware. To the best of our knowledge, this is the first demonstration of in vivo adiabatic two‐dimensional total correlated spectroscopy and fully adiabatic two‐dimensional correlated spectroscopy. It is expected that these methodological developments will advance the in vivo applicability of multi(spectrally)dimensional MRS to reliably identify metabolic biomarkers. Magn Reson Med, 2010. © 2010 Wiley‐Liss, Inc.