What .NET collection provides the fastest search

You should read this blog that speed tested several different types of collections and methods for each using both single and multi-threaded techniques.

According to the results, a BinarySearch on a List and SortedList were the top performers constantly running neck-in-neck when looking up something as a "value".

When using a collection that allows for "keys", the Dictionary, ConcurrentDictionary, Hashset, and HashTables performed the best overall.

If you don't need ordering, try HashSet<Record> (new to .Net 3.5)

If you do, use a List<Record> and call BinarySearch.

In the most general case, consider System.Collections.Generic.HashSet as your default "Contains" workhorse data structure, because it takes constant time to evaluate Contains.

The actual answer to "What is the fastest searchable collection" depends on your specific data size, ordered-ness, cost-of-hashing, and search frequency.

Have you considered List.BinarySearch(item)?

You said that your large collection is already sorted so this seems like the perfect opportunity? A hash would definitely be the fastest, but this brings about its own problems and requires a lot more overhead for storage.