It is better to use Structs when:
You need to store data (and return an output), since the field names are (should be) self-documenting, so you don't need to remember what information you had in column 7 of a cell array. Also, you can easily include a field 'help' in your structure where you can put some additional explanation of the fields, if necessary.
You want to update your code at a later date, replace them with objects without needing to change your code (at least in case you did pre-assignment of your structure). They have the same syntax, but objects will allow you to add more functionality, such as dependent properties (i.e. properties that are calculated on the fly based on other properties).
In the end, it's also a matter of convenience and code clarity. If you prefer to refer your variable elements by number(s) or by name. Then use cell array in the former case and struct array in later.