It has been found that, as a main mechanism for diabetes, insulin resistance may have appeared more than a decade before the onset of diabetes. Therefore, early detection of insulin resistance has vital significance for the early prevention, diagnosis, and treatment of diabetes. The content of intramyocellular lipid (IMCL) in human calf muscle has close and complex relationship with insulin resistance and metabolic disorders and, therefore, is associated with type 2 diabetes mellitus and even a variety of mental diseases. However, the current “gold standard” for IMCL measurement is the invasive biopsy technology, which is not suitable for large-scale basic research and long-term clinical applications. IMCL measurement technology based on proton magnetic resonance spectroscopy and spectroscopic imaging (1H MRSI) provides a radiation-free, non-invasive, and high-precision detection method. More than this, 1H MRSI has been expected to clarify the relationship between IMCL content and insulin resistance, as well as the relationship between insulin resistance and type 2 diabetes mellitus, and has the potential to be applied in clinical practice. This paper describes and summarizes the technical development of 1H MRSI-based IMCL content measurement. It also points out the challenges and the latest solutions of this technique from the aspects of physiological and structural characteristics of calves, muscle fiber direction, the bulk fat distribution, and the demand for precise quantification of IMCL content. In addition to reviewing the latest technical solutions to these problems, we particularly discuss the combination of 1H MRSI with some new technologies such as multi-mode magnetic resonance imaging (MRI) and magnetic resonance fingerprinting spectroscopy (MRFS), which will synergically provide more diversified, multi-dimensional and multi-scale measurement method for high-precision measurement of IMCL.