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I'm running a campaign with a small group of characters avg. level 7. So far they have pounded every "major" encounter they've come across. So I started adjusting the environment to make things a more difficult. They ended up having a far more difficult time getting the group past a waterfall (2 near drownings) than they did with 2 ettercaps, 1 harpoon spider, and 2 large spiders. Now, if I had put 2 or 3 low level goblins at the top of the waterfall with ranged weapons I probably would have killed 1 or 2 people since they would have been tied up with the attackers long enough for the others in the water to drown.
For the spiders, originally I planned the encounter with just 1 harpoon spider and 1 ettercap, but decided to try a bigger challenge. The ettercaps stayed up in the ceiling just out of darkvision range and threw their nets to hold people down while the harpoon spider climbed down to harpoon a PC and reel him back into the ceiling. They took out all the critters pretty easily since the warlock had a spider climb evocation that made him immune to the webs.
After that I started throwing low CR creatures at the party with unique abilities. A choker (MM1) can be pretty tricky. I almost killed the level 6 warlock who wandered off on his own. I've used a couple darkmantles too because their Darkness spell foils darkvision and leads to chaos and mayhem!
Later on they encountered an Avalancher(MM3) who turned the ground under them to mud. They all sank in and it then caused an avalanche, burying 1 of them. Sadly some of them made it out of the mud and killed the avalancher before it could escape.
Throw in some creatures that can use hit and run tactics. My 2 phase spiders did major damage by free-action shifting to the prime, taking 1 bite attack+poison, then using their move action to shift back out. They would then wait a while for the secondary con damage to kick in, then attack again. Eventually the party burned their nest+eggs, so the spiders popped out and fought to the death.
My players can pretty much recognize any Monster Manual creature I throw at them, and though they try not to let it affect their gaming decisions, they already know what type of attacks to expect. I've started putting templates on my creatures to make them a bit spicier. "Wait, the Runehound has 2 tentacles growing out of it too??" "Wait, the troll is poisonous and SMART??" "Look out, a rabbit! Kill it to be safe!"
So far these changes have worked out well. Several near deaths, no real deaths (which is good as we lack anyone that can raise dead), and plenty of surprises.
To sum up - Tactics > more monsters > higher CR.