The aim of this study was to apply loess balls containing effective microorganisms (EM) to the remediation of contaminated harbor sediments, and to thereby elucidate the functions of EM in remediation. Changes in physicochemical, biochemical, and microbiological parameters were measured to monitor the remediation process at a laboratory scale. Treatment with high concentrations of EM stock culture and EM loess balls (4%), and a low concentration of EM loess balls (0.1%) that contained molasses (0.05%) contributed to more rapid removal of malodor. Acetic acid, propionic acid, valeric acid, caponic acid, and lactic acid were rapidly removed in the presence of molasses (0.05% w/w) as a carbon nutrient source, indicating enhanced EM activity by amendment with molasses. Fermentation of molasses by EM showed that more acetic acid was produced compared with other organic acids, and that the majority of organic acids were eventually converted to acetate via intermediate metabolites. Sediment bioremediation tests showed there was no significant difference in eubacterial density with the control and the treatments. However, the density of a Lactobacillus sp. in sediments treated with 0.1% and 4.0% EM loess balls was significantly higher than the control, which indicated the bioaugmentation effect of EM loess balls in the polluted sediments. Treatment with EM loess balls and an appropriate amount of molasses, or other nutrients, will facilitate the remediation of polluted marine sediments by malodor removal, via EM degradation or utilization of offensive organic acids. To our knowledge, this is the first study to remediate contaminated marine (harbor) sediments using EM loess balls and to understand EM function during the bioaugmentation process, both in terms of organic acid metabolism and the dynamics of the engineered microbial community.