The effect of decomposition and diagenesis of sediment organic matter (SOM) on the adsorption of emerging pollutants by the sediment has been seldom addressed. In the present experimental study, artificial sediment was incubated to simulate the natural organic diagenesis process and hence investigate the influence of organic diagenesis on the adsorption of tetracyclines (TCs) by marine sediment. During a period of 4 months of incubation, SOM initially added into the sediment underwent biodegradation and diagenesis. The results showed an early decrease in TC adsorption by the sediment, which was likely caused by the competition between the microbial organic products and TC molecules for the adsorption sites. Afterward, TC adsorption by the sediment increased significantly, which was mainly due to the accumulation of condensed SOM. The experimental results indicate the interactions between TCs and the sediment during the dynamic process of SOM diagenesis. Moreover, the remaining SOM is shown to have an increasing affinity with the antibiotics.