Assuming that you are trying limit the product qty a registered customer who is currently log in can add to their cart.
(This is a one to one relationship, but could easily modify to accomodate many different products and qty per customer)
Create a custom module that will add a field in customer entity, so admin can set the appropriate qty for each customer.
Field name: [ModuleName]_product_id (see Adding attributes to customer entity)
Field name: [ModuleName]_max_cart_qty (see Adding attributes to customer entity)
In (copy files below to your local template folder) and update the qty input field.
/app/design/frontend/base/default/template/catalog/product/view/addtocart.phtml
/app/design/frontend/base/default/template/checkout/cart/item/default.phtml
Change
<input type="text" class="input-text qty" name="qty" id="qty" maxlength="12" value="<?php echo $this->getProductDefaultQty() * 1 ?>" title="<?php echo $this->__('Qty') ?>" />
to (Add a validation class to make sure the qty is less than or equal )
$addValidationClass = '';
if( Customer is login && ModuleName_product_id == $_product->getId() && [ModuleName]_max_cart_qty > 0){
$addValidationClass = ' validate-digits-range-1-' . [ModuleName]_max_cart_qty
}
<input type="text" class="input-text qty<?php echo $addValidationClass; ?>" name="qty" id="qty" maxlength="12" value="<?php echo $this->getProductDefaultQty() * 1 ?>" title="<?php echo $this->__('Qty') ?>" />
If you want to do server-side validation then create a observer for add to cart event, that compare the above logic to the item currently been add to cart