In the study we experimentally examine the influence of elastic properties and surface morphology on the inter-particle friction of natural soil grains. The experiments are conducted with a custom-built micromechanical apparatus and the database is enhanced by testing engineered-reference grains. Naturally-occurring geological materials are characterized by a wide spectrum of mechanical properties (e.g., Young’s modulus) and surface morphology (e.g., roughness), whereas engineered grains have much more consistent characteristics. Comparing to engineered materials, geological materials are found to display more pronounced initial plastic behavior during compression. Under the low normal load range applied in the study, between 1 and 5 N, we found that the frictional force is linearly correlated with the applied normal load, but we acknowledge that the data are found more scattered for natural soil grains, especially for rough and weathered materials which have inconsistent characteristics. The inter-particle coefficient of friction is found to be inversely correlated with the Young’s modulus and the surface roughness. These findings are important in geophysical and petroleum engineering contents, since a number of applications, such as landslides and granular flows, hydraulic fracturing using proppants, and weathering process of cliffs, among others, can be simulated using discrete numerical methods. These methods employ contact mechanics properties at the grain scale and the inter-particle friction is one of these critical components. It is stressed in our study that friction is well correlated with the elastic and morphological characteristics of the grains.