Like Joe MacBu sez, Indian shops are filled to the brim with spices. Bharat Bazaar I think is now called Samosa House - They have samosas that have no equal in this part of town - it's because they roast and grind the spices that go into their samosas, as well as all of their other prepared foods. They have most of their spices against the west wall in their shop, but good luck getting out of there without picking up some food to go. They have something that looks like the equivalent of a giant vegetarian meatball in the food case that is deep-fried upon ordering. Like the samosas, it's eaten with chutney on the side. Can't remember the name of it but give it a try if you're really hungry.
Check out the Indian shops in Culver City, Artesia or Northridge. While they don't have the selection of Penzey's, the quality is usually good and the prices much cheaper (though you usually have to buy larger sizes, you won't necessarily be spending more). Particularly good for cumin, coriander, turmeric, black pepper, cayenne, mustard seeds, etc.
India Sweets and Spices
9409 Venice Blvd.
3126 Los Feliz Blvd.
11510 West Washington Blvd
What spices are you looking for? I know that some places such as Wild Oats markets have some spices available from big jars that you can get whatever quantity you need. I think Whole Foods does this as well, and yet another place is Nicole's in South Pasadena.
If you're looking for commerical sized/priced containers of herbs/spices/etc, let me know, as I can refer you to somebody that has excellent quality products for restaurants & hotels.