My experience, from best to worst:
1. NFCU
1. Discover
3. Amex
4. USAA
5. Capital One
6. GE
7. BofA
NFCU and Discover: No wait times. Knowledgable, courteous, and professional US-based CSR's.
Amex: CSR quality can be inconsistent. They get things done.
USAA: Other than the whole "we can't PC because it's against the law" line, they're okay.
Capital One: Long wait times, CSR's read from scripts, some processes that should be simple are convoluted.
GE: Foreign CSR's who work from a script.
BofA: I won't even go there.
Lately, I have been reading about how Company A is horrible because they speak in a foreign language or Company B keeps passing the buck and can't give you a straight forward answer.
On the other side, Company C has excellent CSR service and they are trained well to answer your questions - leaving you happier than before your called - OR Company D who hands out nice CLIs without interrogating you about every little detail in your credit reports.
So here's the big question -- In your experience, who should be in the top 2 positions for BEST Customer Service and why did you put them in those positions? (I'm asking about "Major CC Names" and not startup "bad-credit" CSRs like Credit One of Fingerhut - sorry, that's another discussion for another day.)
I would love to hear your really good experiences and BAD ones too! Anything goes. 
Here's the nominations (Not in any particular order.)
Citi
Chase
Wells Fargo
American Express
Discover
Barclays
First National Bank of Omaha aka FNBO
Capital One
US Bank
Bank of America
Your TOP 2 are:
1.
2.
@northface28 wrote:Barclays
Discover
Why do you like Barclays Northface? I head they are hard core mean. 
Among my CC issuers:
Grade: A+
Amex. No one even comes close.
Grade: A
Discover.
Chase.
Grade: B+
Capital One.
Citibank.
Grade: B
Bank of America.
Barclay.
Synchrony.
Comenity.
Target RED (TD Bank).
Grade: C
If any bank gets a C, then that would probably more a reflection of the USER than the BANK. Sure banks screw up every now and then, but 99% of the complaints about the banks are really user error. Yeah, I'm pointing my fingers at YOU! 