Previous studies have reported promising antimicrobial efficacy for the essential oils and solvent extracts of several indigenous Pelargonium species. This study aimed to determine if any pharmacological interaction (e.g. synergism or antagonism) exists between the volatile and non-volatile components when the different fractions were investigated. The antimicrobial activity of the following fractions were tested; the essential oil prepared by hydrodistillation (EO), non-volatile fraction (NV), prepared by extraction of plant material remaining in the distilling apparatus (having no or negligible volatile constituents) and solvent extracts prepared from fresh (FC) and dried (DC) plant material containing both volatile and non-volatile constituents. Pelargonium quercifolium oil was dominated by p-cymene (42.1%) and viridiflorol (16.9%), while P. graveolens and P. tomentosum oil had high levels of isomenthane (84.0 and 58.8% respectively). Menthone was noted as a major constituent in the P. tomentosum EO sample. It was evident from the results that the presence of volatile constituents in the three species; P. graveolens, P. quercifolium and P. tomentosum is generally not a pre-requisite for antimicrobial activity. The most significant variations of antimicrobial activity were noted for P. tomentosum where poorer activity was noted for the FC and EO fractions against Bacillus cereus and Candida albicans. Studies on Staphylococcus aureus, however, showed the converse, where best activity was noted for the FC fraction (3.0 mg/mL). For P. quercifolium, the DC fraction indicated a notable increase in anti-staphylococcal activity (2.0 mg/mL) when compared with the FC (8.0 mg/mL) and EO (16.0 mg/mL) fractions. For P. tomentosum, the FC fraction indicated much lower antimicrobial activity (against both B. cereus and C. albicans) when compared with all other fractions, suggesting that the essential oils may impact negatively on the antimicrobial activity when tested against these two pathogens.