The LAS Dataset toolbar in ArcMap does not provide any automated classification solutions. The classification that is available through the Profile viewer was meant solely for the facilitation of supervised classification, where you would make a selection and assign the appropriate class code.
In ArcGIS Desktop 10.4 and ArcGIS Pro 1.2, 3D Analyst provides the Classify LAS Ground tool which can be used to obtain a very good classification of ground points on many types of terrain. The freely available 3D Sample Tools package also provides tools for classifying ground and building points using a TIN based methodology. If portions of your data lays in areas where the above-ground returns only contain vegetation, you may want to consider running the Classify LAS By Height tool to assign the vegetation codes based on their height from the ground.