Yes, it is possible, and in some cases, required to have Vcontrol at a higher voltage than Vin.
For example, if you are looking to achieve the lowest dropout, you need to have Vcontrol at a higher level than Vin. For example, with a Vin of 4.1V and Vout of 3.6V, the Vcontrol pin will need to be approx 1.3V above Vout (i.e. Vcontrol = 4.9V) to ensure dropout. The required delta between Vin and Vcontrol will vary depending on the operating temp and load so it is important to check the graphs from page 6 of the datasheet below.