Building on the answers by @Regexident & @Max, I came up with the following methods:
@implementation NSString (SSToolkitAdditions)
#pragma mark Trimming Methods
- (NSString *)stringByTrimmingLeadingCharactersInSet:(NSCharacterSet *)characterSet {
    NSRange rangeOfFirstWantedCharacter = [self rangeOfCharacterFromSet:[characterSet invertedSet]];
    if (rangeOfFirstWantedCharacter.location == NSNotFound) {
        return @"";
    }
    return [self substringFromIndex:rangeOfFirstWantedCharacter.location];
}
- (NSString *)stringByTrimmingLeadingWhitespaceAndNewlineCharacters {
    return [self stringByTrimmingLeadingCharactersInSet:
            [NSCharacterSet whitespaceAndNewlineCharacterSet]];
}
- (NSString *)stringByTrimmingTrailingCharactersInSet:(NSCharacterSet *)characterSet {
    NSRange rangeOfLastWantedCharacter = [self rangeOfCharacterFromSet:[characterSet invertedSet]
                                                               options:NSBackwardsSearch];
    if (rangeOfLastWantedCharacter.location == NSNotFound) {
        return @"";
    }
    return [self substringToIndex:rangeOfLastWantedCharacter.location+1]; // non-inclusive
}
- (NSString *)stringByTrimmingTrailingWhitespaceAndNewlineCharacters {
    return [self stringByTrimmingTrailingCharactersInSet:
            [NSCharacterSet whitespaceAndNewlineCharacterSet]];
}
@end
And here are the GHUnit tests, which all pass of course:
@interface StringCategoryTest : GHTestCase
@end
@implementation StringCategoryTest
- (void)testStringByTrimmingLeadingCharactersInSet {
    NSCharacterSet *letterCharSet = [NSCharacterSet letterCharacterSet];
    GHAssertEqualObjects([@"zip90210zip" stringByTrimmingLeadingCharactersInSet:letterCharSet], @"90210zip", nil);
}
- (void)testStringByTrimmingLeadingWhitespaceAndNewlineCharacters {
    GHAssertEqualObjects([@"" stringByTrimmingLeadingWhitespaceAndNewlineCharacters], @"", nil);
    GHAssertEqualObjects([@"\n \n " stringByTrimmingLeadingWhitespaceAndNewlineCharacters], @"", nil);
    GHAssertEqualObjects([@"\n hello \n" stringByTrimmingLeadingWhitespaceAndNewlineCharacters], @"hello \n", nil);
}
- (void)testStringByTrimmingTrailingCharactersInSet {
    NSCharacterSet *letterCharSet = [NSCharacterSet letterCharacterSet];
    GHAssertEqualObjects([@"zip90210zip" stringByTrimmingTrailingCharactersInSet:letterCharSet], @"zip90210", nil);
}
- (void)testStringByTrimmingTrailingWhitespaceAndNewlineCharacters {
    GHAssertEqualObjects([@"" stringByTrimmingLeadingWhitespaceAndNewlineCharacters], @"", nil);
    GHAssertEqualObjects([@"\n \n " stringByTrimmingLeadingWhitespaceAndNewlineCharacters], @"", nil);
    GHAssertEqualObjects([@"\n hello \n" stringByTrimmingTrailingWhitespaceAndNewlineCharacters], @"\n hello", nil);
}
@end
I submitted a GitHub pull request to SSToolkit with these methods added.