General opposites:
* Uncontentedly
* Dissatisfiedly
* Unhappily
* Restlessly
* Uneasily
More specific opposites:
* Anxiously (if the context is about feeling anxious)
* Angrily (if the context is about feeling angry)
* Sadly (if the context is about feeling sad)
* Miserably (if the context is about feeling miserable)
Ultimately, the best opposite for "contentedly" will depend on the specific meaning you want to convey.