Walley, F. L., Gillespie, A. W., Adetona, A. B., Germida, J. J. and Farrell, R. E. 2014. Manipulation of rhizosphere organisms to enhance glomalin production and C-sequestration: Pitfalls and promises. Can. J. Plant Sci. 94: 1025-1032. Arbuscular mycorrhizal fungi (AMF) reportedly produce glomalin, a glycoprotein that has the potential to increase soil carbon (C) and nitrogen (N) storage. We hypothesized that interactions between rhizosphere microorganisms, such as plant growth-promoting rhizobacteria (PGPR), and AMF, would influence glomalin production. Our objectives were to determine the effects of AMF/PGPR interactions on plant growth and glomalin production in the rhizosphere of pea (Pisum sativum L.) with the goal of enhancing C and N storage in the rhizosphere. One component of the study focussed on the molecular characterization of glomalin and glomalin-related soil protein (GRSP) using complementary synchrotron-based N and C X-ray absorption near-edge structure (XANES) spectroscopy, pyrolysis field ionization mass spectrometry (Py-FIMS), and proteomics techniques to characterize specific organic C and N fractions associated with glomalin production. Our research ultimately led us to conclude that the proteinaceous material extracted, and characterized in the literature, as GRSP is not exclusively of AMF origin. Our research supports the established concept that GRSP is important to soil quality, and C and N storage, irrespective of origin. However, efforts to manipulate this important soil C pool will remain compromised until we more clearly elucidate the chemical nature and origin of this resource.