As in like a Helm of Opposite Alignment? Actually outright changing alignment so the character actually becomes evil, not merely detecting?
The Helm of Opposite Alignment is probably the simplest way. You get a DC 15 will save to prevent it, otherwise it totally swaps your alignment. LG to CE, etc.
The only thing I know of is the Helm of Opposite Alignment.
Do you want to make them detect as evil, or do you want them to actually become evil? For the former is easy, and there's at least half a dozen spells and probably a fair number of items that can do that. The latter is much more difficult and usually requires very, very powerful magic.
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If you happen to know a cleric of an evil deity Imbue with aura would make them count as evil for all purposes for the duration of the spell.
There's a reasonable interpretation based on the reading of the atonement spell that if you take evil actions while controlled (dominate, gaes, etc.) you become evil.
If the atoning creature committed the evil act unwittingly or under some form of compulsion, atonement operates normally at no cost to you.
There's a reasonable interpretation based on the reading of the atonement spell that if you take evil actions while controlled (dominate, gaes, etc.) you become evil.
You don't simply become evil, you just have something that you should atone for. "You can eventually become evil" might be a more reasonable way to put it.
I believe there are some high-CR monsters with ways to make somebody evil. It's usually conditional, though- if they freely agree to have a wish granted (or some such thing), then they become evil. That sort of thing. Gate or a sufficiently high level or boosted Planar Ally/Binding spell can get you access to that.
Life of Crime (Ultimate Intrigue) doesn't change somebody's alignment, but it's a permanent spell that forces a save every hour or briefly be compelled to commit a crime. It also does a fair job of driving them to avoid getting the curse removed, and makes the removal hard enough without that.
This is an aside, please do not let this thread devolve into a "What a paladin should or shouldn't do" thread.
If a paladin uses an ability to make a creature evil just so that they are able to smite them, as a GM I would tell him that is a huge breach of his paladin code.
While Imbue With Aura can make them detect as evil, and for some spell effects to be tagged as evil, it won't work with Smite Evil since that does not work on detect but actual alignment.
For an easier method of detecting evil, how about Infernal Healing? While active, they detect as evil.
/cevah
Some alternate rules and requires the game mastery guide, but there is always insanity. If you could use bestow curse to give someone psychosis, or another personality, that could do the trick. Also, the GM can rule alignment shift, like if you chain someone into a box where they have to kill to survive. Traumatic events can cause insanity, and could at the least rewire the brain for survival, no matter the cost... This does depend on the GM but maybe if you use modify memory you can make people think they killed someone, and slowly they start to... Well you get the rest. Slight chance I read too much Lovecraft.
Not exactly something you could inflict on others, but the Master Spy Prestige Class can detect as certain alignments, and are vulnerable to targeting based on alignment. I guess the next question is, "Is there a spell I could use to give people class features and force them to use it?" No. There is not.