Use the Counter.most_common() method, it'll sort the items for you:
>>> from collections import Counter
>>> x = Counter({'a':5, 'b':3, 'c':7})
>>> x.most_common()
[('c', 7), ('a', 5), ('b', 3)]
It'll do so in the most efficient manner possible; if you ask for a Top N instead of all values, a heapq is used instead of a straight sort:
>>> x.most_common(1)
[('c', 7)]
Outside of counters, sorting can always be adjusted based on a key function; .sort() and sorted() both take callable that lets you specify a value on which to sort the input sequence; sorted(x, key=x.get, reverse=True) would give you the same sorting as x.most_common(), but only return the keys, for example:
>>> sorted(x, key=x.get, reverse=True)
['c', 'a', 'b']
or you can sort on only the value given (key, value) pairs:
>>> sorted(x.items(), key=lambda pair: pair[1], reverse=True)
[('c', 7), ('a', 5), ('b', 3)]
See the Python sorting howto for more information.