Accelerator mass spectrometry (AMS) is the most sensitive method for measuring 129I in environmental samples available today, with a detection limit of about 10–15 for 129I/127I. A drawback of the technique is the time-consuming chemical separation required to prepare AMS targets from raw samples. This step significantly limits applications requiring rapid analyses and large numbers of samples, for example, in monitoring studies associated with nuclear accidents. This work introduces a direct method for 129I measurements by AMS that does not require chemical separation. In this approach, stable iodine (127I) is added to a matrix of niobium (Nb) powder and mixed with dried raw sample. This mixture is pressed directly into a sputter target for AMS analysis. Two types of environmental samples have been tested in this work, seaweed and sediment. No anomalous behavior was noted in the Cs+ sputtering behavior of the targets prepared from these materials. The 129I/127I ratios and 129I concentrations measured by this rapid method were found to be in agreement with reported values that used a conventional AMS method for the same material. Based on our findings, we expect that such rapid measurements can be applied to a wide variety of materials, in addition to seaweed and sediment, as long as the sputtering-induced adverse effects do not prevent the stable operation of the ion source. The method is especially useful for screening large numbers of samples before more precise analyses are made.