Episodic memories consist of semantic information coupled with a rich array of contextual detail. Here, we investigate the neural processes by which information about the sensory context of a learning event is "bound" to the semantic representation of the to-be-encoded item. We present evidence that item-context binding during encoding is mediated by frontoposterior electroencephalographic (EEG) phase locking within and between hemispheres in the theta (4-8 Hz) band. During a task in which subjects encoded words in different font colors, later memory for the word was associated with sustained frontal theta activity and frontoposterior theta-band coherence, primarily within the left hemisphere. When the word-color association was later successfully retrieved, however, neurons synchronized their theta-band responses bilaterally in a more sustained fashion, particularly during the latter part of the stimulus epoch (>800 ms). Our results confirm the importance of functional coupling between frontal and posterior regions for successful encoding. One interpretation of these data is hemispheric contributions to item and context encoding may be asymmetric, with left hemisphere coherence facilitating semantic processing of an item and right hemisphere coherence facilitating processing of sensory context. Theta-band coherence may be an important mechanism by which brain networks exchange information during learning.