Walking is the original form of transportation, and pedestrians have always made up a significant share of transportation system users. In contrast to motorized traffic, which has to move on precisely defined lanes and follow strict rules, pedestrian traffic is not heavily regulated. Moreover, pedestrians have specific characteristics—in terms of size and protection—which make them much more vulnerable than drivers. In addition, the difference in speed between pedestrians and motorized vehicles increases their vulnerability. All these characteristics, together with the large number of pedestrians on the road, lead to many safety problems that professionals have to deal with. One way to tackle them is to model pedestrian behavior using microsimulation tools. Of course, modeling also raises questions of reliability, and this is also the focus of this paper. The aim of the present research is to contribute to improving the reliability of microsimulation models for pedestrians by testing the possibility of applying neural networks in the model calibration process. Pedestrian behavior is culturally conditioned and the adaptation of the model to local specifics in the calibration process is a prerequisite for realistic modeling results. A neural network is formulated, trained and validated in order to link not-directly measurable model parameters to pedestrian crossing time, which is given as output by the microsimulation tool. The crossing time of pedestrians passing the road on a roundabout entry leg has been both simulated and calculated by the network, and the results were compared. A correlation of 94% was achieved after both training and validation steps. Finally, tests were performed to identify the main parameters that influence the estimated crossing time.