Based on the chart 100A is at the high end of what 4AWG can support for short wire lengths, but should be fine. It sounds like you already have wire of that size, which is great, so I'd recommend going with either an 80A or 100A breaker depending on how much power you need. The picture in post #25 of this thread actually shows 4AWG wire and a 100A breaker.
Keep in mind that the breaker should be mounted as close to the positive terminal of the battery as possible to minimize the length of unprotected wire (between the battery and the breaker). In fact, you can get breakers that mount directly to the battery post as shown in post #9.